Engineering surface dipoles on mixed conducting oxides with ultra-thin oxide decoration layers

Matthäus Siebenhofer (), Andreas Nenning, Christoph Rameshan, Peter Blaha, Jürgen Fleig and Markus Kubicek ()
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Matthäus Siebenhofer: Institute of Chemical Technologies and Analytics
Andreas Nenning: Institute of Chemical Technologies and Analytics
Christoph Rameshan: Montanuniversität Leoben
Peter Blaha: Institute of Materials Chemistry
Jürgen Fleig: Institute of Chemical Technologies and Analytics
Markus Kubicek: Institute of Chemical Technologies and Analytics

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Improving materials for energy conversion and storage devices is deeply connected with an optimization of their surfaces and surface modification is a promising strategy on the way to enhance modern energy technologies. This study shows that surface modification with ultra-thin oxide layers allows for a systematic tailoring of the surface dipole and the work function of mixed ionic and electronic conducting oxides, and it introduces the ionic potential of surface cations as a readily accessible descriptor for these effects. The combination of X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) illustrates that basic oxides with a lower ionic potential than the host material induce a positive surface charge and reduce the work function of the host material and vice versa. As a proof of concept that this strategy is widely applicable to tailor surface properties, we examined the effect of ultra-thin decoration layers on the oxygen exchange kinetics of pristine mixed conducting oxide thin films in very clean conditions by means of in-situ impedance spectroscopy during pulsed laser deposition (i-PLD). The study shows that basic decorations with a reduced surface work function lead to a substantial acceleration of the oxygen exchange on the surfaces of diverse materials.

Date: 2024
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DOI: 10.1038/s41467-024-45824-9

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